Ultrafast third-harmonic spectroscopy of single nanoantennas fabricated using helium-ion beam lithography

Metallic nanoantennas are able to spatially localize far-field electromagnetic waves on a few nanometer length scale in the form of surface plasmon excitations ^1-3. Standard tools for fabricating bowtie and rod antennas with sub-20 nm feature sizes are Electron Beam Lithography or Ga-based Focused Ion Beam (FIB) Milling. These structures, however, often suffer from surface roughness and hence show only a limited optical polarization contrast and therefore a limited electric field localization. Here, we combine Ga-and He-ion based milling (HIM) for the fabrication of gold bowtie and rod antennas with gap sizes of less than 6 nm combined with a high aspect ratio. Using polarization-sensitive Third-Harmonic (TH) spectroscopy, we compare the nonlinear optical properties of single HIM-antennas with sub-6-nm gaps with those produced by standard Ga-based FIB. We find a pronounced enhancement of the total TH intensity of more than three in comparison to Ga-FIB antennas and a highly improved polarization contrast of the TH intensity of 250:1 for Heion produced antennas ⁴. These findings combined with Finite-Element Method calculations demonstrate a field enhancement of up to one hundred in the few-nanometer gap of the antenna. This makes He-ion beam milling a highly attractive and promising new tool for the fabrication of plasmonic nanoantennas with few-nanometer feature sizes.